AtmosphericPollutionResearch6(2015)376Ͳ381

Short Communication

Atm spheric Pollution Research

www.atmospolres.com 
Biomass burning emissions contaminate winter snowfalls in urban
Beijing: A case study in 2012
ChaoYou1,2,ShaopengGao1,ChaoXu1,2
1
KeyLaboratoryofTibetanEnvironmentChangesandLandSurfaceProcesses,InstituteofTibetanPlateauResearch,ChineseAcademyofSciences,Beijing
100101,China
2
UniversityofChineseAcademyofSciences,Beijing100049,China

ABSTRACT 
Threemonosaccharideanhydrideslevoglucosan,mannosanandgalactosan weredetectedinwintersnowfallsamples
of 2012inurbanBeijing.Concentrationsofthreeisomersvaryfrom0.15to54.43ngmL–1,withanaveragevalueof
10.49ngmL–1.Levoglucosanisthemostabundantcomponent.Wintersnowfallsarecontaminatedbybiomassburning
emissions seriously in urban Beijing. The main sources are softwood and crop residue burnings around Beijing from
lateautumntoearlywinter,whilelong–rangetransportofbiomassburningemissionscontributemoreduringthelate
winter.Concentrationsofmonosaccharideanhydridesinsnowfallsamplesmaybeaffectedbybothtopographyandthe
meteorologicalconditionsaroundurbanBeijing.
 
Keywords:Biomassburningaerosols,levoglucosan,snowchemistry,airpollution,urbanBeijing CorrespondingAuthor:
ChaoYou 
:+86Ͳ15117982072
:youchao@itpcas.ac.cn


ArticleHistory:
Received:26August2014
Revised:26October2014
Accepted:26October2014

doi:10.5094/APR.2015.041

1.Introduction
 particles has a complex composition in urban Beijing. More than
Air pollution has been a widespread topic in recent years
(Akimoto, 2003; Huang et al., 2014). Aerosols and greenhouse
gasesarethetwomainairpollutants(Akimoto,2003).Aerosolscan
significantlyaltertheEarth’sradiationbyscatteringandabsorbing
solar radiation, and impact microphysical characteristics of cloud
droplets (Ramanathan et al., 2001; Gyawali et al., 2009). AtmoͲ
sphericBrownClouds(ABCs)caused by anthropogenic aerosolsin
South Asia has been received public attention due to the unclear
effectsonregionalandglobalclimatesystemandhydrologicalcycle
(Ramanathanetal.,2001;RamanathanandCrutzen,2003).Similar
phenomenawerealsoobservedatdensely–populatedregionslike
Central America, Brazil, the Mediterranean and North China in
recentyears(RamanathanandCrutzen,2003;Lietal.,2010).
 However, previous studies mainly focused on records of
Biomass burning (BB) emissions contribute to more than half
ofthecarbonaceousaerosols(includingbothelementalcarbonand
organiccarbon)allovertheworld(Jacobsonetal.,2000;Gyawaliet
al.,2009).ThisismoreseriousinChina,e.g.urbanBeijing(Lietal.,
2010;Chengetal.,2013).Severalstudiessuggestedthatairquality
in Beijing was impacted significantly by BB emissions all year
around, and winter was the most remarkable time (Wang et al.,
2006a;Chengetal.,2013;Yuetal.,2013).Burningofcropresidue
(includewheat–strawandcornstalk)andfirewoodwerehighlighted
astwomainsourcesoforganicaerosolsinurbanBeijingfromlate
autumn to winter (Wang et al., 2009; Yu et al., 2013). Aerosol
samples collected from urban Beijing showed high concentrations
oforganicmatterduringwintertime(Wangetal.,2006a;Zhanget
al., 2008; Huang et al., 2014). The organic matter in aerosol
one hundred kinds of organic compounds were identified in
aerosolsamplescollectedfrom urbanBeijing (Wangetal., 2006a;
Wang et al., 2006b). Polycyclic aromatic hydrocarbons (PAHs), n–
alkanes, fatty acids and alcohols, polyols/poly acids, dicarboxylic
acidsandsaccharideshavebeenconsideredtobethemainorganic
components(Wangetal.,2006b).Amongvariouskindsoforganic
compounds,levoglucosananditsisomersshowedsimilarvariation
patterns to traditional BB tracer K+ all year around (Cheng et al.,
2013).Levoglucosanaccountsabout90%oftotalidentifiedsugars
inwinteraerosolsinurbanBeijing(Zhangetal.,2008;Chengetal.,
2013). These studies confirmed that levoglucosan and its isomers
couldbeusefulbiomarkersforBBstudiesinurbanBeijing.

monosaccharideanhydrides(MAs)inaerosols(Wangetal.,2006b;
Zhangetal.,2008;Chengetal.,2013).Consideringoftheirspecific
sourcesandcharacteristics,theseMAscanbeidealbiomarkersfor
BB studies in aqueous samples (You et al., 2014). In this study,
levoglucosan,mannosan,galactosanweredetectedsimultaneously
usingGasChromatography/MassSpectrometry(GC/MS)methodin
wintersnowfallsamplescollectedfromurbanBeijing.Thepossible
impactofBBonsnowfallsamplesinurbanBeijingwasalsoanalyzed.

2.ExperimentandMethods

Snow samples were collected at The Campus of Institute of
Psychology, Chinese Academy of Science (40°00഻N, 116°22഻E). The

©Author(s)2015.ThisworkisdistributedundertheCreativeCommonsAttribution3.0License.
 You et al. – Atmospheric Pollution Research (APR)

sampling site is located at central lawn of the campus, and there
are no obvious BB sources within 5 km around. Fresh snow was
collectedinaplasticcontainerwithpolyethylene(PE)bagswhenit
began to snow. Samples were compacted into pre–cleaned
polyethylene terephthalate (PET) bottles within half an hour after
snowfallstopped.Therewerefoursnowsamplescollectedintotal
fromNovember2012toJanuary2013(pleaseseedetailedsample
informationinTable1).Sampleswerekeptfrozenatatemperature
of–20°Cbeforeanalysis.Samplesweredriedbyfreeze–dryingfor
at least 24 h, and then extracted three times using an ultrasonic
method for 30min in a 5mL mixture of dichloromethane/
methanol=4/1(v/v). After concentrated and dried completely
under high purity N2, samples were silylated by N–methyl–N–
trimethylsi–lyltrifluoroacetamide containing 1% trimethylchloroͲ
silane before GC/MS analysis. Silylated extracts were analyzed
usingaTraceGC2000gaschromatographconnectedtoaPolarisQ
iontrapmassspectrometer.Moredetailedinformationaboutthe
sample preparation and determination can been found in a
previousstudy(Youetal.,2014).
 6.86to563.07ngm–3,withanaverageof261.65ngm–3.Resultsin
Table1.Meteorologicaldatainfoursnowfallevents
Ta(°C) RHb(%) SEWc(mm) WSd(ms–1) WDe
th
Nov4 2012 2.9 82 48.9 5.2 Nf
th
Dec12 2012 –2.1 69 0.2 1.6 SWWg
st
Dec21 2012 –4.6 71 0.6 0.8 SWWg
th
Jan20 2012 –2.5 72 2 0.9 SEh
a
Temperature,bRelativehumidity,cSnowequivalentwater,dWindspeed,
Winddirection,fNorth,gSouthWestWest,hSoutheast
e
 1210ngm–3, with an average of 403ngm–3 (Fu et al., 2008).
MeteorologicaldataisfromtheChinaMeteorologicalAdminisͲ
tration. To identify the BB source regions more clearly, backward
trajectorieswerecalculatedbyHYSPLITmodelandMODIShotspot
data (1km×1km, AFD, 2013) were used (Justice et al., 2002).
Because the lifetime of BB aerosols are usually no more than a
week (Ramanathan and Crutzen, 2003), seven days backward air
mass trajectories were used in this study. The matrixes (centered
withsamplesite,0.1°×0.1°,9 points)insteadofsingle–pointswere
used to identify the potential about BB sources around sampling
site in HYSPLIT model. The height of the atmospheric boundary
layer(ABL)varied from300to 600mabove groundlevel(AGL)in
urbanBeijingduringwintertime(Guinotetal.,2007).Theheightof
100m (green line), 500m (blue line) and 3000m (red line) AGL
wassettoanalyzethebackwardtrajectoriesinABL,thetopofABL
andaboveABL,respectively.

3.ResultsandDiscussion
 Figure 1). The ratio of levoglucosan/mannosan is 10.32 for
3.1.BBaerosolscontaminatewintersnowfallsamples
 ratios are consistent with results of aerosol studies in Beijing
Concentrations of three isomers in winter snowfall samples
ranged from 0.15 to 54.43ngmL–1, with an average value of
10.49ngmL–1.Levoglucosanwithanaveragevalueof25.30ngmL–1,
accounts for more than 80% of the total detected MAs. Detailed
results can be seen in Table2. Levoglucosan, mannosan and
galactosancanonlybegeneratedfromthedegradationofcellulose
and hemicellulose when the burning temperature is higher than
300°C (Simoneit et al., 1999). Therefore, those three MAs are
specific biomarkers for BB aerosols. The existence of those three
MAs indicates that winter snowfall samples in urban Beijing are
substantiallycontaminatedbyBBemissions.
 burningonNovember4th2012andsnowfallonJanuary20th2013
Previousobservationandmodelingresultsindicatedthatwet
depositionwasthedominantsinkfororganicmatter,especiallyat
middle and low latitude regions (Hu et al., 2013). The following
equation is used to transform the concentrations of MAs in snow



377
samples to their related concentrations in the atmosphere
(Davidsonetal.,1993):

‫׋‬௔ ൌ ʌ௔ ൈ ‫׋‬௦ Ȁʘ (1)

whereC࡭isconcentrationofspecies(ngmо3)intheatmosphere,p࡭
isairdensity(gm–3)underthestandardtemperatureandpressure
(0°C and 1.01×105Pa, in this study the value of 1293gm–3 is
used),CsisconcentrationofMAs(nggо1,actuallyequalstongmL–1)
in snow, andʘis the scavenging ratio for specific species by
snowfall. The value 125 was recommended as a worldwide mean
of ʘ for both black carbon and organic matter (Jacobson, 2004),
and this value is used to estimate the concentrations of MAs
approximatelyinthisstudy.

Concentrations of MAs in the atmosphere estimated by the
Equation (1) in four snowfall events are shown in Table2. Total
concentrationsofMAsvariedfrom16.01to683.15ngm–3,withan
averageof325.61ngm–3.Levoglucosanconcentrationsrangedfrom
thisstudycanbecomparabletopreviousaerosolstudiesinurban
Beijing. Concentration of levoglucosan was about 575ngm–3 in
PM2.5 aerosol samples in winter (Zhang et al., 2008). ConcenͲ
trations of levoglucosan varied from 60 to 1940ngm–3, with a
meanvalueof590ngm–3,andconcentrationsofmannosanvaried
from50to190ngm–3intypicalwinteraerosolsamples(Chenget
al., 2013). However, the estimated concentrations of MAs in this
study are much higher than previous aerosol studies at other
regions in China. Concentrations of levoglucosan in aerosols at
MountTaiduringthewheatstrawburningperiodvariedfrom88to
Concentrations of levoglucosan in winter aerosols in Guangzhou
varied from 57.9 to 269.3ngm–3, with an average value of
176.6ngm–3(Maetal.,2009).Theconcentrationsoflevoglucosan
atHongKongrangedfrom26.2to133.7ngm–3(Sangetal.,2011).
Those comparable results evidently proved that snowfall samples
inurbanBeijingwereseriouslycontaminatedbyBBemissions.

3.2.IdentificationofBBsources

Previous studies suggested different ratios of MAs (e.g.
levoglucosan/mannosan)canbeusefultoidentifytheBBsourcesin
urban Beijing (Cheng et al., 2013). Although degradation happens
duringthetransportprocess,theimpactofthedegradationonthe
ratios among MAs has been considered to be limited (Hu et al.,
2013).Differentsnowsamplesdisplaydistinctratiosoflevglucosan/
mannosan, indicating that snowfall samples in urban Beijing are
contaminated by various sources of BB in winter (Table 2 and
December12thand8.86forDecember21st2012,respectively.The
(levoglucosan/mannosan with an average of 9.01±1.47 for typical
winter samples) (Cheng et al., 2013). Snowfall samples on
December 12th and December 21st 2012 may be contaminated by
mixed aerosols released from softwood and crop residual
(Figure1).Hardwood,grassandleafburningmayalsoactasnon–
negligible sources. However, ratios of levoglucosan/mannosan on
November 4th 2012 and January 20th 2013 are different from
previous aerosol studies, which indicate snowfalls on these two
daysarecontaminatedbydifferentBBemissionsources.Compared
with previous studies (please see detailed data in the Supporting
Material,SM),thepossiblesourcesaresoftwood,needleandduff
may be contaminated by hardwood burning. This classification
method may have some uncertainties, because it is based on
limited statistical analysis results from previous studies. However,
this method can help us to understand the contaminations of
snowfallsamplescausedbyBBaerosolsatsomeextent.
 You et al. – Atmospheric Pollution Research (APR) 378

Table2.ConcentrationsofMAsinfoursnowfallsamples(ngmL–1)
Nov4th2012 Dec12th2012 Dec21st2012 Jan20th2013
Galactosan 0.73 4.99 5.47 1.66
Mannosan 0.15 4.39 6.14 1.20
Levoglucosan 0.66 45.31 54.43 0.77
Levogluocsan/Mannosan 4.41 10.32 8.86 0.64
EstimatedconcentrationsofMAsintheatmosphereforfoursnowfallevents(ngm–3)
Galactosan 7.60 51.64 56.54 17.17
Mannosan 1.56 45.41 63.54 12.41
Levoglucosan 6.86 468.71 563.07 7.95
TotalMAs 16.02 565.76 683.15 37.53

(a) (b)



Figure1.(a)Levoglucosan/mannosanratiosamongvariouskindsofBBsourcesfromdifferentreferences.Thecentralbaristhemedian,andthe
boxshowsthefirstandthethirdquartiles,respectively.Thewhiskershowsthemaximumandminimumvalues.Thehollowblocksymbols
indicatearithmeticalmeans.Thecrossesindicateextremevalues.DetaileddatacanbefoundintheSM.(b)Thedependenceoflevoglucosanon
mannosaninwintersamplesinurbanBeijing,thegraydots(k1,b1,r12)areaerosolsamplesfromChengetal.(2013),theblackdots(k2,b2,r22)are
snowsamplesinthisstudy.

The results based on HYSPLIT backward air mass trajectories distinctregionsatdifferentaltitudes(Figure2d).Pollutantsmainly
indicate potential emission source regions (Figure2). The come from northern China and nearby regions at the low layers
northeastern China is seen as the major source region for BB (100 and 500 m), while pollutants may come from southwestern
aerosolsnearthesurface(100and500m)onNovember4th2012, China at 3000 m AGL. Southwestern China is mainly covered by
while the Jiaodong Peninsula and the Eastern Coastal China are largeareasofbroad–leaveddeciduousforestandbunchgrass.Fires
seen as the two major source regions at high altitude (3000m, occur during January 2013 at Yunnan, Sichuan, Henan and some
Figure2a). During late September to early November, the other provinces (XHN, 2013) along the trajectories due to the dry
atmosphereisgreatlyinfluencedbytheburningofagriculturecrop weather conditions. Additionally, burning incense and joss paper
residueandfallenleavesinNorthernChina.Burningfumescanbe during the Spring Festival is prevalent in those regions, which can
transportedabovetheABL,andthuscanbetransportedtoregions alsocontributetolong–rangetransportofBBaerosols.
farawayfromtheemissionsources.Similarrecordsofcropresidue 
burning were reported by previous studies in urban Beijing and 3.3.Possibleimpactfactors
regions nearby (Zhang et al., 2008; Cheng et al., 2013). The dry 
weatherisprevalentsincelateautumnatmostregionsofnorthern Previous studies suggested that aerosols released from BB
China (Zhai et al., 2005), which increases the risks of forest and couldpersistintheatmospherefromhourstoseveraldays(China
grasslandfires.TheBBsourceregionsfortwosnowfallsamplesin etal.,2013).Thetransportpathwaysareimportanttounderstand
December2012aredifferentfromsnowfallonNovember4th 2012 the effects of BB aerosols on snowfall samples in urban Beijing.
(Figure2band2c).BBaerosolsmainlyreleasefromNorthernChina Urban Beijing is located at the foothill of northeast–southwest
and Mongolia and sometimes from as far as central Asia in oriented Yanshan Mountains. Prevailing winds are mostly from
December 2012. Although only few forest or steppe fires occur in southeast and southwest during the investigated period (Table 1).
winter time at those regions, firewood burning for heating and ThisisconsistentwithresultofHYSPLITmodel.Theorientationof
cookingareprevalentinnorthernChina,MongoliaandcentralAsia mountain provides possible pathways for BB aerosols. The
in winter (Wang et al., 2006a; Zhang et al., 2008). It is also distribution of surrounding mountains form the semi–basin
noticeablethatBBemissionsfromNortheasternChinamaybeone topographyofurbanBeijing,whichfacilitatestheaccumulationof
ofthemostimportantsourcesforsnowfallonDecember12th2012, BB aerosols (Wu et al., 2011). The accumulated BB aerosols can
especiallyforaerosolstransportedatlowaltitude(100and500m leadtohigherconcentrationsofMAsinurbanBeijing.
AGL). The result based on HYSPLIT backward air mass trajectories 
indicates that BB contaminations on January 20th 2013 are from 
 You et al. – Atmospheric Pollution Research (APR) 379



(a) (b)

(c) (d)

Figure2.SevenͲdaybackwardairmasstrajectoriesbasedontheHYSPLITmodelforBBsourcesidentification.Thegreenlinesstandfor100 mAGL,blue
linesstandfor500mAGLandredlinesstandfor3000mAGL.ThereddotsarefirehotspotsfromMODIS.(a)November4th2012,
(b)December12th2012,(c)December21st2012and(d)January20th2013.

The dispersion of BB aerosols is influenced by many other
factors in addition to emission sources. The meteorological
conditions are thought to be the most important factors which 5HODWLYH+XPLGLW\
affectthediffusionprocess(Huetal.,2013;Sunetal.,2013).Due
to limited samples, we can only give the extrapolation but not
statistical results. High concentrations of MAs in snow samples
occur with low precipitation and low wind speed (Figure 3). This
mightbebecausesnowfallcandilutetheBBaerosols,whichleads
tolowerconcentrationsofMAsinsnowsamples.Previousstudies
of marine aerosols found that concentration of levoglucosan was
stronglyinfluencedbytheeffectofprecipitationscavengingatlow
latitude regions (Hu et al., 2013). The dispersion of BB aerosols is
faster in windy days than calm days (Sun et al., 2013), leading to
higher concentrations of MAs in calm days. Previous studies
indicatedthatfasterdecayoflevoglucosanwasobservedathigher
relative humidity conditions in laboratory (Hennigan et al., 2010).
Concentrations of MAs in snow samples and relative humidity
show an inverse variation trendency in urban Beijing during the
studyperiod(Figure3).Thisresultindicatesthatrelativehumidity
might even affect the oxidation of MAs after deposition, which is
important to understand the effectiveness of levoglucosan as
Figure3.Influenceofmajormeteorologicalfactors(precipitation,wind
biomarker in sediments. However, this hypothesis is deduced by
speedandrelativehumidity)onconcentrationsofMAsinfoursnowfall
preliminaryresultsinthisstudy,whichneedsmoredatatoproveit.
events.



 You et al. – Atmospheric Pollution Research (APR)

4.Conclusions
 indicateshighlevelsofbiomassburningaerosolsoveroceansfromthe
ThisstudyreportedBBsignalsinsnowfallsamplesusingMAs
records in urban Beijing during 2012 winter period. Snowfall
samples are contaminated by both regional emissions and long–
range transport aerosols released from various kinds of BB. The
possible BB sources are revealed by ratios of levoglucosan/
mannosan, HYSPLIT model and MODIS fire hotspots. The concenͲ
trations of MAs show significant temporal variations. The
topographymayaffectthepathwaysofBBaerosols.Meteorological
conditions may affect the dispersion of BB aerosols and the
concentrationsofMAsinsnowfallsamples.Thisstudyishelpfulto
understand the contribution of BB emissions to air pollution in
urbanBeijing,andisalsohelpfultotheenvironmentalsignificance
ofBBemissions.
 accounting for soot's feedback to snow and sea ice albedo and
Acknowledgments
 D21201.
ThisstudyissupportedbyNationalNaturalScienceFoundation
ofChina(41190081),KnowledgeInnovationProgramoftheChinese
Academy of Sciences (KZCX2–YW–T11) and Chinese Academy of
Sciences Third Pole Environment Program (GJHZ0906). Thanks
NOAA for providing HYSPLIT model, NECP/NCAR data and MODIS
fireaccountsdata.ThanksChinaMeteorologicalAdministrationfor
meteorologicaldata.
 Ma,S.X.,Wang,Z.Z.,Bi,X.H.,Sheng,G.Y.,Fu,J.M.,2009.Compositionand
Theauthorsthanktheeditorandthreeanonymousreviewers
fortheirvaluablecommentsandsuggestions.
 Ramanathan, V., Crutzen, P.J., 2003. New directions: Atmospheric brown
SupportingMaterialAvailable
 Ramanathan,V.,Crutzen,P.J.,Kiehl,J.T.,Rosenfeld,D.,2001.Atmosphere–
Ratios among three monosaccharide anhydrides (MAs) from
different sources (Table S1). This information is available free of
chargeviatheinternetathttp://www.atmospolres.com.
 S.,Zhang,Z.S.,Zhang,T.,Hu,M.,2011.Levoglucosanenhancementin
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